Surfactant-assisted hydrothermally synthesized MoS_2 samples with controllable morphologies and structures for anthracene hydrogenation  

表面活性剂辅助水热制备形貌结构可控的MoS2及其蒽加氢性能(英文)

作　　者：李敏[1,2,3] 王冬娥[2] 李佳鹤[2,3] 潘振栋[2] 马怀军[2] 姜玉霞[2,3] 田志坚[2,4] 陆安慧[1] 

机构地区：[1]大连理工大学化工学院精细化工国家重点实验室,辽宁大连116024 [2]中国科学院大连化学物理研究所洁净能源国家实验室(筹),辽宁大连116023 [3]中国科学院大学,北京100049 [4]中国科学院大连化学物理研究所催化基础国家重点实验室,辽宁大连116023

出　　处：《Chinese Journal of Catalysis》2017年第3期597-606,共10页催化学报（英文）

基　　金：supported by the National Natural Science Foundation of China(21303186);the Strategic Priority Research Program of the Chinese Academy of Sciences(XDA07020300)~~

摘　　要：MoS_2 samples with controllable morphologies and structures were synthesized using surfactantassisted hydrothermal processes.The effects of surfactants（PEG,PVP,P123,SDS,AOT,and CTAB）on the morphologies and structures of MoS_2 samples were investigated.The results revealed that spherical,bulk-like,and flower-like MoS_2 particles assembled by NH4~＋-intercalated MoS_2 nano-sheets were synthesized.The morphologies of the MoS_2 samples and their structures（including the slab length and the number of stacked layers） of MoS_2 nano-sheets in these samples could be controlled by adjusting the surfactants.Mono-dispersed spherical MoS_2 particles could be synthesized with PEG via the creation of MoS_2 nano-sheets with slab lengths shorter than 15 nm and fewer than six stacked layers.Possible formation mechanisms of these MoS_2 samples created via surfactant-assisted hydrothermal processes are proposed.Further,the catalytic activities of MoS_2 samples for anthracene hydrogenation were evaluated in a slurry-bed reactor.The catalyst synthesized with the surfactant PEG exhibited the highest catalytic hydrogenation activity.Compared with the other catalysts,it had a smaller particle size,mono-dispersed spherical morphology,shorter slab length,and fewer stacked layers;these were all beneficial to exposing its active edges.This work provides an efficient approach to synthesize transition metal sulfides with controllable morphologies and structures.随着原油资源重质化和劣质化的加剧以及对清洁燃料油品需求的不断增加,将重质油加工成清洁燃料成为现代炼厂面临的挑战.悬浮床加氢是重质油转化为清洁液体燃料的先进技术,其核心难题是高效加氢催化剂的开发.MoS_2在石油化工领域油品加氢提质研究中表现出非常好的催化加氢性能.MoS_2晶体结构中有两种面:沿S-Mo-S层间的剥离面,又称基面,化学性质稳定;沿Mo-S的断裂面,又称棱面,具有大量的不饱和键,化学性质不稳定,可做催化活性中心.由于MoS_2结构和形貌对其物理化学性能有重要影响,所以通过合理设计和调控MoS_2的结构和形貌可增加暴露的催化活性位,进而改善其催化性能.本文以七钼酸铵和硫代乙酰胺为原料,水合肼做还原剂,采用不同表面活性剂(包括PEG,PVP,P123,SDS,AOT和CTAB)辅助的水热合成法制备了结构及形貌可控的MoS_2,并提出不同表面活性剂条件下MoS_2催化剂的生长机理,进一步研究了重油模型化合物稠环芳烃蒽的催化加氢性能.结果表明,在不同表面活性剂辅助的条件下分别制得了由MoS_2纳米片组装而成的球形、块状和花状的MoS_2产物;通过改变表面活性剂种类可调变MoS_2纳米片的长度、堆积层数、层间距以及最终产物的形貌.在PEG或PVP辅助下得到了球形MoS_2产物,其中MoS_2纳米片长<15 nm,堆积层数<6.在PEG辅助下制备的球形MoS_2粒径约为250 nm,尺寸均一且分散性好.在PVP辅助下MoS_2粒径在200–450 nm,粒径分布范围宽且有明显团聚.在P123或SDS辅助下得到了团聚较明显的块状微米级MoS_2产物.在P123辅助下得到的MoS_2纳米片长<15 nm,层数<6.在SDS辅助下制备的MoS_2纳米片长>20 nm,堆积层数>8.在AOT或CTAB辅助下得到团聚比较严重的花状微米级MoS_2产物,其中MoS_2纳米片长>20 nm,堆积层数>8.另外,水热反应过程中,高温高压的环境促进了反应体系中游离的NH_4^+插入到MoS_2层状�

关 键 词：Molybdenum sulfide Surfactant-assisted Controllable morphology Mono-dispersed Active edges Anthracene hydrogenation 

分 类 号：O643.36[理学—物理化学]